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Understanding Cycling Mechanisms and...

Dawson, Andrew Akash.

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Understanding Cycling Mechanisms and Degradation in High-Capacity Electrodes for Ion Battery Applications.

紀錄類型:	書目-電子資源 : Monograph/item
正題名/作者:	Understanding Cycling Mechanisms and Degradation in High-Capacity Electrodes for Ion Battery Applications./
作者:	Dawson, Andrew Akash.
出版者:	Ann Arbor : ProQuest Dissertations & Theses, : 2023,
面頁冊數:	141 p.
附註:	Source: Dissertations Abstracts International, Volume: 85-03, Section: B.
Contained By:	Dissertations Abstracts International85-03B.
標題:	Chemistry. -
電子資源:	https://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=30639405
ISBN:	9798380349161

Understanding Cycling Mechanisms and Degradation in High-Capacity Electrodes for Ion Battery Applications.
Dawson, Andrew Akash.

Understanding Cycling Mechanisms and Degradation in High-Capacity Electrodes for Ion Battery Applications. - Ann Arbor : ProQuest Dissertations & Theses, 2023 - 141 p.

Source: Dissertations Abstracts International, Volume: 85-03, Section: B.

Thesis (Ph.D.)--University of California, Los Angeles, 2023.

Lithium-ion batteries are essential energy storage devices for modern-day technology and for creating a more sustainable future. One limitation is the energy density. This dissertation describes materials to increase the energy density of batteries, design principles to encourage reversibility, and examines how the structure changes with lithiation and delithiation. The first part focuses on nanoporous tin antimonide (NP-SbSn) as an anode material. NP-SbSn performs well with only 1% capacity fade after 100 cycles. To make structure-property relationships, we use a combination of transmission x-ray microscopy (TXM), X-ray diffraction (XRD), and transmission electron microscopy (TEM). We compare these results with previous results on nanoporous tin to show that the use of an intermetallic stabilizes the structure and discover that the mechanism of lithiation involves amorphization, unlike bulk SbSn. Because of the increased stability of SbSn vs Sn, NP-SbSn is cycled with sodium, a harder material to cycle with. There is more structural degradation, but we obtain 85% capacity retention of after 100 cycles, To increase structural stability, a surface coating of aluminum oxide was added resulting in less structural damage under sodiation when compared to uncoated NP-SbSn.The second part of the dissertation focuses on nanoporous antimony (NP-Sb). NP-Sb is used to study the effects of non-crystalline intermediates when cycling because we observed amorphization during lithiation of NP-SbSn. Unusually, Sb cycles similarly with sodium as with lithium. When cycled against lithium, NP-Sb has crystalline intermediates and amorphous intermediates, when cycled against sodium. Through XRD and TXM, we show how crystalline changes can have large effects on macro- and meso-scale structure. Also, we reveal synergistic effects when amorphous intermediates are combined with mesoporosity.Lastly, we synthesize novel, icosahedral boron clusters as a cathode material through solid-state methods, atypical for boron cluster syntheses. These clusters are cross-linked with disulfides, resulting in redox active sulfur and clusters. The cluster's role is two-fold: the cross-linked nature prevents sulfur dissolution and provide capacity. We observe solid-state redox of the cluster, for the first time, and sulfur with reversible cycling. Cluster and sulfur redox are confirmed with operando Raman spectroscopy.

ISBN: 9798380349161Subjects--Topical Terms:

516420
Chemistry.
Subjects--Index Terms:

Alloy anodes

Understanding Cycling Mechanisms and Degradation in High-Capacity Electrodes for Ion Battery Applications.
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300 $a 141 p.
500 $a Source: Dissertations Abstracts International, Volume: 85-03, Section: B.
500 $a Advisor: Tolbert, Sarah H.
502 $a Thesis (Ph.D.)--University of California, Los Angeles, 2023.
520 $a Lithium-ion batteries are essential energy storage devices for modern-day technology and for creating a more sustainable future. One limitation is the energy density. This dissertation describes materials to increase the energy density of batteries, design principles to encourage reversibility, and examines how the structure changes with lithiation and delithiation. The first part focuses on nanoporous tin antimonide (NP-SbSn) as an anode material. NP-SbSn performs well with only 1% capacity fade after 100 cycles. To make structure-property relationships, we use a combination of transmission x-ray microscopy (TXM), X-ray diffraction (XRD), and transmission electron microscopy (TEM). We compare these results with previous results on nanoporous tin to show that the use of an intermetallic stabilizes the structure and discover that the mechanism of lithiation involves amorphization, unlike bulk SbSn. Because of the increased stability of SbSn vs Sn, NP-SbSn is cycled with sodium, a harder material to cycle with. There is more structural degradation, but we obtain 85% capacity retention of after 100 cycles, To increase structural stability, a surface coating of aluminum oxide was added resulting in less structural damage under sodiation when compared to uncoated NP-SbSn.The second part of the dissertation focuses on nanoporous antimony (NP-Sb). NP-Sb is used to study the effects of non-crystalline intermediates when cycling because we observed amorphization during lithiation of NP-SbSn. Unusually, Sb cycles similarly with sodium as with lithium. When cycled against lithium, NP-Sb has crystalline intermediates and amorphous intermediates, when cycled against sodium. Through XRD and TXM, we show how crystalline changes can have large effects on macro- and meso-scale structure. Also, we reveal synergistic effects when amorphous intermediates are combined with mesoporosity.Lastly, we synthesize novel, icosahedral boron clusters as a cathode material through solid-state methods, atypical for boron cluster syntheses. These clusters are cross-linked with disulfides, resulting in redox active sulfur and clusters. The cluster's role is two-fold: the cross-linked nature prevents sulfur dissolution and provide capacity. We observe solid-state redox of the cluster, for the first time, and sulfur with reversible cycling. Cluster and sulfur redox are confirmed with operando Raman spectroscopy.
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650 4 $a Materials science. $3 543314
650 4 $a Analytical chemistry. $3 3168300
653 $a Alloy anodes
653 $a Amorphous anodes
653 $a Boron cluster cathodes
653 $a Lithium ion battery
653 $a Sodium ion battery
653 $a Transmission x-ray microscopy
690 $a 0485
690 $a 0794
690 $a 0486
710 2 $a University of California, Los Angeles. $b Chemistry 0153. $3 2096181
773 0 $t Dissertations Abstracts International $g 85-03B.
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791 $a Ph.D.
792 $a 2023
793 $a English
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